A correlation-based inversion approach for satellite-borne aerosol remote sensing
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The purpose of this campaign was to deploy an instrument payload collocated with a suite of in situ and remote-sensing aerosol instruments at the urban site at the La Porte, Texas Municipal Airport during the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) in Houston, Texas. The payload was designed to characterize the physicochemical properties, mixing state, and size-resolved vertical fluxes of aerosols. Deployed aerosol instruments associated with the flux measurements included three condensation particle counters (CPCs) with different lower cutoff diameters ( D > 2.5 nm, D > 10 nm, and D > 40 nm), a single-particle soot photometer (SP2) measuring refractory black carbon, and a portable optical particle spectrometer (POPS) measuring the optical size distribution (~180 nm < D < ~5000 nm). A 10-m flux tower hosted a sonic anemometer (SONIC) for vertical velocity measurements. In addition, a humidified tandem differential mobility analyzer (HTDMA) was deployed to measure the growth factors and hygroscopicity parameter of 15-50 nm-sized particles in order to constrain the composition of compounds responsible for modal aerosol growth during new particle formation/growth events. Finally, a radial differential mobility analyzer (RDMA) was deployed to extend the size distribution measurement to 5 nm.
Aerosol particles cool the climate by scattering solar radiation and by acting as cloud condensation nuclei. Higher temperatures resulting from increased greenhouse gas levels have been suggested to lead to increased biogenic secondary organic aerosol and cloud condensation nuclei concentrations creating a negative climate feedback mechanism. Here, we present direct observations on this feedback mechanism utilizing collocated long term aerosol chemical composition measurements and remote sensing observations on aerosol and cloud properties. Summer time organic aerosol loadings showed a clear increase with temperature, with simultaneous increase in cloud condensation nuclei concentration in a boreal forest environment. Remote sensing observations revealed a change in cloud properties with an increase in cloud reflectivity in concert with increasing organic aerosol loadings in the area. The results provide direct observational evidence on the significance of this negative climate feedback mechanism.
Abstract Integrated measurements of aerosol, radiation, cloud, and turbulent transport in the planetary boundary layer (PBL) are essential for understanding and modeling climate and air quality. Here, we developed a new technique for the identification of convective turbulent regions and deriving the vertical distribution of aerosol turbulent mass fluxes within PBL. The algorithm uses retrievals from coherent Doppler lidars and a high spectral resolution lidar. The technique was applied to study particle mass fluxes over 2 months (November–December 2020) during the campaign conducted at the DOE Atmospheric Radiation Measurement Southern Great Plains (SGP) site in Lamont, Oklahoma. The algorithm developed here is capable of continuously deriving vertically resolved (curtains) aerosol mass fluxes. Our data analysis shows that at the site, the 30‐min averaged fluxes at 135 m above the surface were mainly positive (upward) at ∼1 μg m −2 s −1 , suggesting that the surface is the primary source of the particle mass supplied to the boundary layer at the SGP site. Analyses of the individual case studies have revealed that not all the derived fluxes can be linked to surface emissions. Both positive and negative values in a range of ±5 μg m −2 s −1 can be caused by convective thermals interacting between the residual layer and the mixed layer and by rotation of the horizontal wind with the height. Large erroneous negative fluxes can also be caused by drizzling/precipitating clouds. We anticipate that the application of the current technique will lead to a more realistic representation of aerosol mass budgets and bidirectional mixing rates.
The cloud condensation nuclei (CCN) concentration at cloud base is the most relevant measure of the aerosol that influences droplet formation in clouds. Since the CCN concentration depends on supersaturation, a more general measure of the CCN concentration is the CCN spectrum (values at multiple supersaturations). The CCN spectrum is now measured at the surface at several U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility observatories and by the ARM Mobile Facility (AMF) but is not measured at the cloud base. Rather than rely on expensive aircraft measurements for all studies of aerosol effects on clouds, a way to project CCN observations made at the surface to cloud base is needed. Remote sensing of aerosol extinction provides information about the vertical profile of the aerosol but cannot be directly related to the CCN concentration because the aerosol extinction is strongly influenced by humidification, particularly near cloud base. Ghan and Collins (2004) and Ghan et al. (2006) propose a method to remove the influence of humidification from the extinction profiles and tie the “dry extinction” retrieval to the surface CCN concentration, thus estimating the CCN profile. This methodology has been implemented as ARM’s Retrieved Number Concentration of CCN (RNCCN) Profile Value-Added Product (VAP).
The ACT-America project is a NASA Earth Venture Suborbital-2 mission designed to study the transport and fluxes of greenhouse gases. The open and freely available ACT-America data sets provide airborne in situ measurements of atmospheric carbon dioxide, methane, trace gases, aerosols, clouds, and meteorological properties, airborne remote sensing measurements of aerosol backscatter, atmospheric boundary layer height and columnar content of atmospheric carbon dioxide, tower-based measurements, and modeled atmospheric mole fractions and regional carbon fluxes of greenhouse gases over the Central and Eastern United States. In this study, we conducted 121 research flights during five campaigns in four seasons during 2016–2019 over three regions of the US (Mid-Atlantic, Midwest and South) using two NASA research aircraft (B-200 and C-130). We performed three flight patterns (fair weather, frontal crossings, and OCO-2 underflights) and collected more than 1,140 h of airborne measurements via level-leg flights in the atmospheric boundary layer, lower, and upper free troposphere and vertical profiles spanning these altitudes. We also merged various airborne in situ measurements onto a common standard sampling interval, which brings coherence to the data, creates geolocated data products, and makes it much easier for the users to perform holistic analysis of the ACT-America data products. Here, we report on detailed information of data sets collected, the workflow for data sets including storage and processing of the quality controlled and quality assured harmonized observations, and their archival and formatting for users. Finally, we provide some important information on the dissemination of data products including metadata and highlights of applications of ACT-America data sets.
Abstract There is a lack of satellite‐based aerosol retrievals in the vicinity of low‐topped clouds, mainly because reflectance from aerosols is overwhelmed by three‐dimensional cloud radiative effects. To account for cloud radiative effects on reflectance observations, we develop a Convolutional Neural Network and retrieve aerosol optical depth (AOD) with 100–500 m horizontal resolution for all cloud‐free regions regardless of their distances to clouds. The retrieval uncertainty is 0.01 + 5%AOD, and the mean bias is approximately −2%. In an application to satellite observations, aerosol hygroscopic growth due to humidification near clouds enhances AOD by 100% in regions within 1 km of cloud edges. The humidification effect leads to an overall 55% increase in the clear‐sky aerosol direct radiative effect. Although this increase is based on a case study, it highlights the importance of aerosol retrievals in near‐cloud regions, and the need to incorporate the humidification effect in radiative forcing estimates.
We assessed satellite-retrieved marine aerosol in the western Antarctic Peninsula (WAP) across a 12-year period from coarse-mode aerosol optical depth (AOD C ), often used as a proxy for sea spray aerosol (SSA), and marine aerosol optical depth (MAOD), a newly developed proxy for tropospheric marine aerosol. Across open ocean to coastal regions, daily fluctuations in nighttime and daytime winds, respectively, drove increasing MAOD and AOD C . MAOD depicted strong correlations with wind speed across open ocean and weak correlations in coastal regions. In the open ocean, AOD C exhibited a very weak significant correlation to wind speed and a weak significant correlation to sea surface temperature (SST). We thus observed that warmer SST enhanced the production of SSA, supporting prior studies. This is the first study to assess patterns of AOD C in the WAP. In contrast to the tropical Pacific, seasonal patterns showed that biological activity likely contributed toward MAOD and AOD C magnitudes.
Vertically resolved observations of the temporal evolution of mixed-phase clouds (MPCs) were performed over the central Arctic during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, which lasted from October 2019 to September 2020. The research icebreaker Polarstern , drifting with the pack ice for more than 7 months, mostly at latitudes > 85° N, served as a platform for state-of-the-art remote sensing of aerosols and clouds. The use of the recently introduced dual field-of-view (FOV) polarization lidar technique in combination with the well-established lidar-radar retrieval technique provided, for the first time, a robust instrumental basis to monitor the evolution of the liquid and the ice phase of MPCs and the interplay between the two phases. Two long-lasting Arctic MPC events observed close to the North Pole in mid-winter (December 2019) and late summer (September 2020) are discussed to provide new insight into Arctic MPC evolution processes. In the second part of the article, cloud statistics, covering all seasons of a year, are presented. The focus is on the optical and microphysical properties of the liquid phase. These results are solely derived from the dual-FOV lidar observations. The key findings of the study can be summarized as follows: persistent activation of aerosol particles to form water droplets is of great importance for the longevity of MPCs. The observations confirm that ice formation occurs predominantly via immersion freezing. The field studies suggest that the free tropospheric reservoirs of cloud condensation nuclei (CCN) and of ice-nucleating particles (INPs) were always well filled, i.e., the clouds did not exhaust their supply of activatable and activated particles. The observation of long-lasting MPC events, low ice production rates, and a sufficiently large INP reservoir leads to the recommendation to use a time-dependent immersion freezing parameterization in MPC modeling efforts.
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Vertical profiles of aerosols are inadequately observed and poorly represented in climate models, contributing to the current large uncertainty associated with aerosol–cloud interactions. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) aircraft field campaign near the Azores islands provided ample observations of vertical distributions of aerosol and cloud properties. Here we utilize the in situ aircraft measurements from the ACE-ENA and ground-based remote-sensing data along with an aerosol-aware Weather Research and Forecast (WRF) model to characterize the aerosols due to long-range transport over a remote region and to assess their possible influence on marine-boundary-layer (MBL) clouds. The vertical profiles of aerosol and cloud properties measured via aircraft during the ACE-ENA campaign provide detailed information revealing the physical contact between transported aerosols and MBL clouds. The European Centre for Medium-Range Weather Forecasts Copernicus Atmosphere Monitoring Service (ECMWF-CAMS) aerosol reanalysis data can reproduce the key features of aerosol vertical profiles in the remote region. The cloud-resolving WRF sensitivity experiments with distinctive aerosol profiles suggest that the transported aerosols and MBL cloud interactions (ACIs) require not only aerosol plumes to get close to the marine-boundary-layer top but also large cloud top height variations. Based on those criteria, the observations show that the occurrence of ACIs involving the transport of aerosol over the eastern North Atlantic (ENA) is about 62 % in summer. For the case with noticeable long-range-transport aerosol effects on MBL clouds, the susceptibilities of droplet effective radius and liquid water content are -0.11 and +0.14, respectively. When varying by a similar magnitude, aerosols originating from the boundary layer exert larger microphysical influence on MBL clouds than those entrained from the free troposphere.
The evolution of disciplinary silos and increasingly narrow disciplinary boundaries have together resulted in one-sided approaches to the study of land-atmosphere interactions—a field that requires a bi-directional approach to understand the complex feedbacks and interactions that occur. The integration of surface flux and atmospheric boundary layer measurements is therefore essential to advancing our understanding. The Land-Atmosphere 2021 workshop (held virtually, June 10-11, 2021) involved almost 300 participants from around the world and promoted cross-discipline collaboration by way of talks from invited speakers, moderated discussions, breakout sessions, and a virtual poster session. The workshop focused on five main theme areas: “big picture” overview, instrumentation and remote sensing, modeling, water, and aerosols and clouds. In talks and breakout groups, there were frequent calls for more AmeriFlux sites to be instrumented for boundary layer height measurements, and for the development of some “super sites” where profiling instruments would be deployed. There was further agreement on the need for the standardization of various datasets. There was also a consensus that funding agencies need to be willing to support the sorts of large projects (including associated instrumentation) which can drive interdisciplinary work. Early-career scientists, in particular, expressed enthusiasm for working across disciplinary boundaries but noted that there need to be more financial support and training opportunities so they would be better prepared for interdisciplinary work. Investment in these career development opportunities would enable today's cohort of early-career scientists to advance the frontiers of interdisciplinary work over the next couple of decades.
Permanent and mobile facilities deployed by the ARM program cover a wide range of climatic regions, with a suite of active remote-sensing of cloud and aerosol profiles complemented by comprehensive in-situ measurements of the chemical, physical and optical properties of aerosol measured at the surface. To be able to fully exploit these datasets requires an understanding of the transport from the surface and within the atmosphere, especially within the planetary boundary layer. This requires a method of identifying when the surface and atmosphere are dynamically-linked. Determining the state of the boundary layer, and defining a well-mixed boundary-layer, is therefore suitably described in terms of mixing; here, we will assume that mixing essentially means turbulent mixing. This necessitates accurate measurements of the winds and turbulent mixing in the atmosphere. Doppler lidar is an excellent tool for observing turbulent properties, and ARM has deployed commercially available Doppler lidars at many of the fixed and mobile facilities. Doppler lidars have been shown to provide accurate retrievals of wind and turbulent properties within the boundary layer , however, robust characterization and calculation of the Doppler lidar measurement uncertainties is required before deriving higher level data products.
As the Arctic continues to change and warm rapidly, it is increasingly important to understand the organic carbon (OC) contribution to Arctic aerosol. Biogenic sources of primary and secondary OC in the Arctic will be impacted by climate change, including warming temperatures and earlier snow and ice melt. Here, this study focuses on identifying potential sources and regional influences on the seasonal concentration of organic aerosol through analysis of chemical and isotopic composition. Aerosol samples were collected at two sites on the North Slope of Alaska ($Utqia\dot{g}vik$, UQK, and Oliktok Point, OLK, which is in an Arctic oilfield) over three summers from 2015 to 2017. The elemental carbon (EC) trends at each site were used to understand local combustion influences. Local sources drove EC concentrations at Oliktok Point, where high EC was attributed to oil and gas extraction activity, including diesel combustion emissions. $Utqia\dot{g}vik$ had very low EC in the summer. OC was more similar in concentration and well correlated between the two sites with high contributions of contemporary carbon by radiocarbon apportionment (UQK = 74%, OLK = 63%), which could include both marine and terrestrial sources of contemporary carbon (e.g. primary and secondary biogenic, biomass burning and/or associated SOA, and bioaerosols). OC concentrations are strongly correlated to maximum ambient temperatures on the NSA during the summer, which may have implications for predicting future OC aerosol concentrations in a warming Arctic. Biomass burning was determined to be an episodic influence at both sites, based on interpretation of combined aerosol composition, air mass trajectories, and remote sensing of smoke plumes. The results from this study overall strongly suggests contribution from regional sources of contemporary organic aerosol on the NSA, but additional analysis is needed to better constrain contributions from both biogenic sources (terrestrial and/or marine) and bioaerosol to better understand temperature-related aerosol processes in the Arctic.
The objective of this campaign was to complement the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) User Facility’s Cloud And Precipitation Experiment at kennaook (CAPE-k) in northwest Tasmania by deploying scanning, fixed pointing angle, and in situ aerosol, cloud, and precipitation remote-sensing instruments during the last six months of the experiment. These instruments provided a three-dimensional (3D) context to the second ARM Mobile Facility (AMF2) vertically pointing observations collected at the kennaook Cape Grim (KCG) site and captured a portion of the life cycle of the clouds before and after the passage over the AMF2 vertical column. These 3D cloud measurements will be used in the near future to 1) investigate how the vertical profiles of aerosol and cloud properties are representative of the broader area and how these properties evolve during the portion of the cloud life cycle captured by the scanning instruments, 2) quantify how accurate the cloud fraction derived with assumptions from vertically pointing observations are compared with direct 3D cloud fraction measurements, 3) evaluate cloud fraction and liquid water path in the Australian Community Climate and Earth-System Simulator–Convective-scale (ACCESS-C) forecast model, and 4) evaluate aerosol and cloud products from the European Space Agency/Japanese Aerospace Exploration Agency (ESA/JAXA) Earth Cloud Aerosol Radiation Explorer (EarthCARE) mission using the scanning measurements, offering more chances of exact collocation, thereby complementing the statistical approach we are planning to employ with AMF2 observations for that same purpose.
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Excitation from optically trapped particles is examined through laser-induced breakdown spectroscopy following interactions with mJ-level fs pulses. Optical emissions from sub-ng ablation of precisely positioned cupric oxide microparticles are used as a method to spatially resolve laser–particle interactions resulting in excitation. External focusing lenses are often used to change the dynamics of nonlinear self-focusing of fs pulses to form laser filaments or, alternatively, to form very intense air plasmas. Given the significant implications external focusing has on laser propagation and plasma conditions, single-particle emissions are studied with focusing lenses ranging from 50 to 300 mm. It is shown that, while single particles are less excited at longer focal lengths due to limited energy transfer through laser–particle interactions, the cooler plasma results in a lower thermal background to reveal resolved single-shot emission peaks. Furthermore, by developing an understanding in the fundamental interaction that occurs between single particles and fs pulses and filaments, practical improvements can be made for atmospheric remote sensing of low-concentration aerosols.
This report summarizes the results of a U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility workshop held in November 2019 to advance a science-based strategy for ARM’s aerosol measurement program. This was the second such workshop since the Aerosol Measurement Science Group (AMSG) was chartered in 2015 to enhance coordination of ARM observations of aerosols and atmospheric trace gases with the needs of ARM users. The results presented here reflect the AMSG’s focus in recent years on science-based strategies that will contribute to the increased use of ARM data to fulfill its mission of improving process representations and predictability in climate models. Sessions held during the workshop range from interfacing with models through aerosol sampling strategies to calibration protocols and data products. The strategies set forth here were also developed to be directly relevant to ARM’s updated Decadal Vision. The AMSG workshops have been designed to recommend actions that will enable ARM to evolve and continue to meet its mission. To that end, the AMSG will develop an actionable plan from the recommendations outlined here. Some are well defined and can reasonably be accomplished in the short term. Others are less definite or of a larger scope that calls for a longer-term implementation. Further discussion will be required to develop and prioritize actionable items related to such areas. Task teams comprising the appropriate expertise and perspective from the AMSG and other members of the community will be formed to achieve this outcome. Some particular topics are recognized as high priority, so plans are underway to develop task teams and to hold follow-on discussions to address them. Four areas currently being considered for short, focused discussion are 1) aerosol measurements on the North Slope of Alaska, 2) improving data usability for modeling, 3) strategies for advancing remote sensing, vertical profiling, and distributed measurements of aerosols, and 4) aerosol sampling strategies at existing ARM sites to provide intensive modes of operation to promote data usage for process and modeling studies.